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US20030157002A1 - Apparatus for the conversion of hydrocarbons - Google Patents

Apparatus for the conversion of hydrocarbons Download PDF

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Publication number
US20030157002A1
US20030157002A1 US10/203,928 US20392803A US2003157002A1 US 20030157002 A1 US20030157002 A1 US 20030157002A1 US 20392803 A US20392803 A US 20392803A US 2003157002 A1 US2003157002 A1 US 2003157002A1
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US
United States
Prior art keywords
reactor
gasses
catalyst
conversion
pressure
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Abandoned
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US10/203,928
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English (en)
Inventor
Eleonoor Andel
Erik Middelman
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Individual
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Individual
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Priority claimed from NL1014404A external-priority patent/NL1014404C1/nl
Priority claimed from NL1015916A external-priority patent/NL1015916C1/nl
Priority claimed from NL1015917A external-priority patent/NL1015917C1/nl
Application filed by Individual filed Critical Individual
Publication of US20030157002A1 publication Critical patent/US20030157002A1/en
Abandoned legal-status Critical Current

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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F28—HEAT EXCHANGE IN GENERAL
    • F28D—HEAT-EXCHANGE APPARATUS, NOT PROVIDED FOR IN ANOTHER SUBCLASS, IN WHICH THE HEAT-EXCHANGE MEDIA DO NOT COME INTO DIRECT CONTACT
    • F28D9/00—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall
    • F28D9/04—Heat-exchange apparatus having stationary plate-like or laminated conduit assemblies for both heat-exchange media, the media being in contact with different sides of a conduit wall the conduits being formed by spirally-wound plates or laminae
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/2415—Tubular reactors
    • B01J19/243—Tubular reactors spirally, concentrically or zigzag wound
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C—CHEMISTRY; METALLURGY
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    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/386—Catalytic partial combustion
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    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/48—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents followed by reaction of water vapour with carbon monoxide
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    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
    • C01B3/58—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction
    • C01B3/583—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction the reaction being the selective oxidation of carbon monoxide
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material
    • H—ELECTRICITY
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    • H01M8/0662—Treatment of gaseous reactants or gaseous residues, e.g. cleaning
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B01J2219/00076—Controlling the temperature by indirect heating or cooling employing heat exchange fluids with heat exchange elements inside the reactor
    • B01J2219/00085—Plates; Jackets; Cylinders
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    • B01J2219/0015—Controlling the temperature by thermal insulation means
    • B01J2219/00155—Controlling the temperature by thermal insulation means using insulating materials or refractories
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    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
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    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
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    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
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    • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
    • C01B2203/0261—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a catalytic partial oxidation step [CPO]
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    • C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
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    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
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    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
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    • C01B2203/0844—Methods of heating the process for making hydrogen or synthesis gas by heat exchange with exothermic reactions, other than by combustion of fuel the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
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    • C01B2203/0866—Methods of heating the process for making hydrogen or synthesis gas by combination of different heating methods
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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Definitions

  • the invention relates to a fuel processor for the conversion of hydrocarbons to hydrogen, and to the conversion process.
  • Fuel processors, or reformers are used for large-scale conversion of natural gas to hydrogen. Hydrogen, or a mixture of hydrogen and other gasses like carbon dioxide and nitrogen produced by fuel processors can be used as a fuel for fuel cells, like polymer electrolyte membrane (PEM) fuel cells.
  • PEM polymer electrolyte membrane
  • the wire mesh stabilizes the flame, and the reaction heat is used for reforming of the remaining hydrocarbons.
  • the method has serious drawbacks for small-scale fuel processors.
  • the high reaction temperature causes insulation problems, and severe heat loss in small fuel processors.
  • the total heat loss being the product of radiation losses, conduction loss and heat loss trough convection
  • the insulation problems necessary use of pure oxygen is unpractical.
  • the object of this invention is to provide a apparatus for the conversion of hydrocarbons to hydrogen rich gas mixtures, that operates at a relatively low temperature, uses air in stead of pure oxygen, can be operated at atmospheric pressure, has a low pressure drop, is compact, has low thermal mass and having high thermal efficiency.
  • this objective is achieved by a apparatus in which heating of the feed gasses, an exothermic reforming reactor, a shift reactor, and cooling of the hot reformed gas stream are integrated in counter flow, in such a way that the feed gasses are heated by the exhaust gasses and by the exothermic CPO reaction and/or the exothermic reaction between Carbon Monoxide and oxygen or the exothermic reaction between hydrogen and oxygen, this heat exchanger having the form of a large number of thermal radiation reflectors that are co-heated by the exothermal of the CPO reaction, and the integrated reactor having the form of a multi-blade spiral, having preferably 4 blades, and between these blades the channels for feed gas (hydrocarbon containing gas), an air containing gas mixture, reformed gas and an empty channel.
  • this heat exchanger having the form of a large number of thermal radiation reflectors that are co-heated by the exothermal of the CPO reaction
  • the integrated reactor having the form of a multi-blade spiral, having preferably 4 blades, and between these blade
  • the inner walls of the channels are coated partly or completely with a catalytically active layer or layers.
  • the construction is elucidated in FIG. 1.
  • the moistened feed gas and the moistened air containing gas are fed to the outer channels of the spiral reactor. Both gasses follow the spiraling gas channels, flow to the center of the spiral, and during their flow to the center these gasses are heated by the gas stream that has already reacted., and flows from the heart of the reactor outwards trough its spiraling channel. Thus the in going gas stream is heated, and the out going gas stream is cooled in counter flow. An other effect is cooling of the channel walls that act as radiation shields.
  • the incoming gasses are kept separated until they have reached a temperature that is sufficiently high for a reaction to take place.
  • the blades of the spiral shaped reactor are made from thin sheet metal with a thickness that is preferably less than 1 mm and more than 25 micron, more preferred less than 250 micron, and more than 40 micron. The optimum thickness depends on the material used, the required pressure drop over the reactor, and the size of the reactor. Blade thickness typically lies between 49 and 126 micron. Heat resistant metals and metal alloys like tungsten and tantalum can be used but are expensive. Preferred are stainless steel, like AISI type 316, and alloys of Iron, Chromium, Aluminum and Yttrium. The spiral shaped seals between the blades can be welded, soldered or folded.
  • the thin sheet metal can be coated with suitable coatings.
  • suitable coatings are corrosion resistant metal layers and for example metal oxide coatings.
  • Preferred are metal oxide coatings like; SiO2 optionally comprising also other elements like, but not limited to Tin, Titanium Aluminum, Cerium, Phosphor or Borium. Thickness of the metal oxide layers is in the range of 10 to 1.000.000 nm, typically a few microns.
  • Preferred precursors for these protective coatings are polymers, especially Silicone polymers, preferably cross-linkable Silicone elastomers. An example of such a protective coating is given in example 2.
  • the fuel processor according to the invention contains spiral shaped thin metal blades that are coated single sided or double sided with a catalytically active layer or layers to obtain a reactor with high heat exchange capacity and low pressure drop. Only the sides of the blades in direct contact with the hydrocarbon containing gas an/or the reformate are coated with catalyst.
  • the catalyst layers are preferably applied prior to assembly of the reactor. Application was done by spay coating, brush coating and can be done by most known coating techniques.
  • As precursor for the catalyst carrier silicone elastomers can be used that are subsequently crosslinked and pyrolized in an oxygen containing atmosphere.
  • the active catalyst can be impregnated after pyrolises in the nano porous silicon oxide layer, can be applied directly as a component in the silicone elastomer coating liquid or can be applied in a two step process were first the silicone elastomer is coated and partially or completely cross linked and subsequently swollen by a suitable solvent containing the active catalyst or a precursor for this active catalyst, drying and pyrolizing.
  • the moistening of the feed gasses is also important. Up to 10% of the total heat is necessary for supplying the required amount of water vapor. According to the invention the heat leak of the reformer is used. This is can be done even better if the whole system is operated at atmospheric pressure If the fuel processor is used in combination with a low temperature fuel cell, the moistening is done in two steps. First the heat generated in the fuel cell stack is used, to generate water vapor at a temperature that is below the temperature of the outer shell of the fuel processor, than the water vapor content is further increased by heating the gasses by passing them over the outer shell of the fuel processor that. The outer shell has typically a temperature between 80° C. and 100° C.
  • the fuel processor is preferably operated at or close to atmospheric pressure to obtain high system efficiency, it is according to the invention possible to operate the fuel processor at higher than atmospheric pressure.
  • the spiral shaped reactor as such is not appropriate for operation with a large pressure difference between the spiral shaped reaction chamber and the surrounding atmosphere.
  • This drawback is solved according to this invention by placing the spiral shaped reactor in a pressure resistant chamber as further explained in FIG. 4.
  • a pressure leveling connection between the air channel and the pressure resistant chamber is provided. The pressure in the spiral shaped reactor will be at the same level as the pressure in the surrounding pressure resistant chamber.
  • Startup of the reactor can be done by electrical heating the center of the spiral outside the gas channels, by placing a catalyst coated or catalytically active hot wire inside the gas channels in the center of the spiral or by direct heating of the center with a flame or catalytic burner.
  • the reactor does not contain coordinates inside the gas channels were the distance to the nearest wall is more than 5 mm, this distance being preferably less than 3 mm.
  • the fuel processor of this example was designed for feeding a 1 kWe PEM fuel cell.
  • the reactor/heat exchanger has a unwound length of 2 meter, a height of 0,3 meter, contains 3 spiral shaped gas slits between 4 spiral shaped 125 micron thick blades(see FIG. 1), one channel (A) with a height of 2 mm is for the in coming moistened hydrocarbon containing gas stream, one other (B) with a height of 4 mm for the incoming moistened air stream, and the third slit (C) is for the out going reformate having a height of 5 mm.
  • the total height of the 3 slits, including the four blades is thus 9,5 mm.
  • a last reaction step is selective oxidation of the reformate to remove traces of CO.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Energy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Sustainable Development (AREA)
  • Electrochemistry (AREA)
  • Physics & Mathematics (AREA)
  • Thermal Sciences (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Fuel Cell (AREA)
  • Hydrogen, Water And Hydrids (AREA)
US10/203,928 2000-02-17 2001-02-19 Apparatus for the conversion of hydrocarbons Abandoned US20030157002A1 (en)

Applications Claiming Priority (6)

Application Number Priority Date Filing Date Title
NL1014404 2000-02-17
NL1014404A NL1014404C1 (nl) 2000-02-17 2000-02-17 Apparaat voor de omzetting van fossiele brandstoffen in waterstofrijke gasmengsels.
NL1015916 2000-08-11
NL1015916A NL1015916C1 (nl) 2000-08-11 2000-08-11 Apparaat voor de omzetting van fossiele brandstoffen in waterstofrijke gasmengsels met behulp van een katalytisch actieve coating.
NL1015917A NL1015917C1 (nl) 2000-08-11 2000-08-11 Methode voor het aanbrengen van katalytisch actieve lagen.
NL1015917 2000-08-11

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US20030157002A1 true US20030157002A1 (en) 2003-08-21

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EP (1) EP1265811A1 (fr)
WO (1) WO2001060739A1 (fr)

Cited By (5)

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US20050074648A1 (en) * 2003-10-02 2005-04-07 Arthur Alan R. Integrated fuel cell stack and catalytic combustor apparatus, assembly, and method of use
EP1630130A1 (fr) * 2004-08-18 2006-03-01 Shell Internationale Researchmaatschappij B.V. Dispositif pour le traitement de combustible et procédé pour le démarrage dudit dispositif
US20070000173A1 (en) * 2005-06-28 2007-01-04 Michael Boe Compact reforming reactor
US20080020336A1 (en) * 2004-10-13 2008-01-24 Webasto Ag Burner Device with a Porous Body
US20090214910A1 (en) * 2008-02-22 2009-08-27 Ultracell Corporation Low pressure drop fuel processor for use with portable fuel cells

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DE10142794A1 (de) * 2001-08-31 2003-03-20 Ballard Power Systems Katalytische Beschichtung für eine Gaserzeugungseinheit
RU2760381C1 (ru) * 2021-06-09 2021-11-24 Юрий Фёдорович Юрченко Способ пиролитического разложения газообразных углеводородов и устройство для его осуществления

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WO1995010126A1 (fr) * 1993-10-06 1995-04-13 Ceramatec, Inc. Conception modulaire d'empilements de piles a combustible d'oxyde solide cpn/reformateur integre

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US3915125A (en) * 1971-07-16 1975-10-28 Siemens Ag Method for the operation of internal-combustion engines and gas reformer for implementing the method
US3955941A (en) * 1973-08-20 1976-05-11 California Institute Of Technology Hydrogen rich gas generator
US5324452A (en) * 1992-07-08 1994-06-28 Air Products And Chemicals, Inc. Integrated plate-fin heat exchange reformation
US5628931A (en) * 1994-07-07 1997-05-13 Shell Oil Company Process for the preparation of hydrogen and carbon monoxide containing mixtures

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Publication number Priority date Publication date Assignee Title
US20050074648A1 (en) * 2003-10-02 2005-04-07 Arthur Alan R. Integrated fuel cell stack and catalytic combustor apparatus, assembly, and method of use
US7306868B2 (en) * 2003-10-02 2007-12-11 Hewlett-Packard Development Company, L.P. Integrated fuel cell stack and catalytic combustor apparatus, assembly, and method of use
US20080085434A1 (en) * 2003-10-02 2008-04-10 Arthur Alan R Integrated fuel cell stack and catalytic combustor apparatus, assembly, and method of use
US8062803B2 (en) 2003-10-02 2011-11-22 Eveready Battery Company, Inc. Fuel cell system and a method of generating electricity
EP1630130A1 (fr) * 2004-08-18 2006-03-01 Shell Internationale Researchmaatschappij B.V. Dispositif pour le traitement de combustible et procédé pour le démarrage dudit dispositif
US20080020336A1 (en) * 2004-10-13 2008-01-24 Webasto Ag Burner Device with a Porous Body
US7758337B2 (en) * 2004-10-13 2010-07-20 Enerday Gmbh Burner device with a porous body
US20070000173A1 (en) * 2005-06-28 2007-01-04 Michael Boe Compact reforming reactor
US20090214910A1 (en) * 2008-02-22 2009-08-27 Ultracell Corporation Low pressure drop fuel processor for use with portable fuel cells
US8129059B2 (en) * 2008-02-22 2012-03-06 UltraCell, L.L.C. Low pressure drop fuel processor for use with portable fuel cells

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WO2001060739A1 (fr) 2001-08-23

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